Atom probe analysis of electrode materials for Li-ion batteries: challenges and ways forward

Kim, Se‐Ho; Antonov, Stoichko; Zhou, Xuyang; Stephenson, Leigh T.; Jung, Chanwon; El‐Zoka, Ayman A.; Schreiber, Daniel K.; Conroy, Shelly; Gault, Baptiste

doi:10.1039/d1ta10050e

Cited by 30 publications

(32 citation statements)

References 76 publications

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“…[75] In very recent work, atom probe tomography (APT) has been proposed as a complementary technique to TEM, which has shortcomings in Li-containing materials. [76] APT can capture 3D distribution of the light elements including Li, with compositional sensitivity of tens of parts-per-million. Together with APT at the same location as STEM, Chae et.al., demonstrated the evolution of the local Li composition and the corresponding structural changes at the atomic scale in the NMC with subnanometer resolution.…”

Section: Atomistic-scale Measurementsmentioning

confidence: 99%

Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies

Tanim

Weddle

Yang

et al. 2022

Advanced Energy Materials

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Charging lithium‐ion batteries (LiBs) in 10 to 15 min via extreme fast‐charging (XFC) is important for the widespread adoption of electric vehicles (EVs). Lately, the battery research community has focused on identifying XFC bottlenecks and determining novel design solutions. Like other LiB components, cathodes can present XFC bottlenecks, especially when considering long‐term battery life. Therefore, it is necessary to develop a comprehensive understanding of how XFC conditions degrade LiB cathodes. The present article reviews relevant cathode‐focused studies and summarizes the current understanding regarding cathode performance and aging issues under XFC conditions. Dominant aging modes and mechanisms are identified at different length‐scales with electrochemical correlations for LiNixMnyCozO2 (NMC)‐based cathodes. A range of electrochemical techniques and models provide key insights into cathode performance and life issues. A suite of multimodal and multiscale microscopy and X‐ray techniques is surveyed to quantify chemical, structural, and crystallographic NMC‐cathode degradation. Cathode cycle‐life is scaled to equivalent EV miles to illustrate how cathode degradation translates to real‐world scenarios and quantifies cathode‐related bottlenecks that hinder XFC adoption. Finally, the article discusses several cathode cycle‐life aging mitigation strategies with example case studies and identifies remaining challenges.

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Section: Atomistic-scale Measurementsmentioning

confidence: 99%

Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies

Tanim

Weddle

Yang

et al. 2022

Advanced Energy Materials

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“…While these studies demonstrate the value of APT in 3D nanoscale compositional analysis of battery cathodes, the deviation in the measured composition from expected stoichiometry highlights the need to better understand the parametric effect arising from the APT sample preparation and APT data acquisition parameters. In this direction, a recent work by Kim et al reveals the dependency of a variety of sample preparation methodologies on the APT results from NMC811 cathodes. Specifically, in the case of samples prepared by cryogenic PFIB and/or ultrahigh vacuum transfer, they reported the occurrence of an electrostatic field induced by in situ delithiation because of ion migration.…”

Section: Introductionmentioning

confidence: 99%

Nanoscale Compositional Mapping of Commercial LiNi_0.8Co_0.15Al_0.05O₂ Cathodes Using Atom Probe Tomography

Parikh

Chung

et al. 2022

J. Phys. Chem. C

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Nickel-rich cathodes provide improved specific capacity, which leads to higher gravimetric energy density, which, in turn, is critical for electric vehicles. However, poor long-term capacity retention at elevated temperatures/high C rates (the rate of charge and discharge on a battery) stems from material issues: surface phase changes, corrosive side reactions with the electrolyte, ion dissolution, and propagation of cracks. Introducing dopants, developing nanoscale surface coatings, and graded core–shell structures all improved the electrochemical performance of nickel-rich cathodes. However, material-level understanding of the effect of Li composition and distribution in Ni-rich cathodes is limited due to a lack of characterization methods available that can directly image Li at the nanoscale. Hence, it is critical to establish methods such as atom probe tomography (APT) that have both nanometer-scale spatial resolution and high compositional sensitivity to quantitatively analyze battery cathodes. To fully realize its potential as a method for quantitative compositional analysis of commercial Li-ion batteries, we provide a comprehensive description of the challenges in sample preparation and analyze the dependency of the analysis parameters, specifically laser pulse energy on the measured stoichiometry of elements in a high-Ni-content cathode material LiNi0.8Co0.15Al0.05O2 (NCA). Our findings show that the stoichiometry variations cannot be explained by charge–state ratios or Ga implantation damage alone during FIB preparation, indicating that additional factors such as crystallographic orientation may need to be considered to achieve quantitative nanoscale compositional analysis of such battery cathodes using APT.

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“…More recently, Qiu et al have analyzed Au nanoparticles contained in aqueous solution using a graphene encapsulation technique to observe the liquid–NP interface (Qiu et al, 2020). Among these emerging sampling techniques, Kim et al developed the co-electrodeposition of a metal to embed various nanomaterials including freestanding hollow TiO 2 nanowires (Lim et al, 2020), MoS 2 nanosheets (Kim et al, 2020 b ), Li 4 Ti 5 O 12 (Kim et al, 2022), Pd nanoparticles (Kim et al, 2018; Jang et al, 2021), and Pd@Au core@shell nanoparticles (Kim et al, 2020 a ).…”

Section: Introductionmentioning

confidence: 99%

Tracking the Mn Diffusion in the Carbon-Supported Nanoparticles Through the Collaborative Analysis of Atom Probe and Evaporation Simulation

Jung

Jun

Jang

et al. 2022

Microscopy and Microanalysis

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Carbon-supported nanoparticles have been used widely as efficient catalysts due to their enhanced surface-to-volume ratio. To investigate their structure–property relationships, acquiring 3D elemental distribution is required. Here, carbon-supported Pt, PtMn alloy, and ordered Pt3Mn nanoparticles are synthesized and analyzed with atom probe tomography as model systems. A significant difference of Mn distribution after the heat-treatment was found. Finally, the field evaporation behavior of the carbon support was discussed and each acquired reconstruction was compared with computational results from an evaporation simulation. This paper provides a guideline for studies using atom probe tomography on the heterogeneous carbon-supported nanoparticle system that leads to insights toward a wide variety of applications.

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Atom probe analysis of electrode materials for Li-ion batteries: challenges and ways forward

Abstract: The worldwide developments of electric vehicles, as well as large-scale or grid-scale energy storage to compensate the intermittent nature of renewable energy generation has generated a surge of interest in...

Cited by 30 publications

References 76 publications

Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies

Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies

Nanoscale Compositional Mapping of Commercial LiNi_0.8Co_0.15Al_0.05O₂ Cathodes Using Atom Probe Tomography

Tracking the Mn Diffusion in the Carbon-Supported Nanoparticles Through the Collaborative Analysis of Atom Probe and Evaporation Simulation

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Atom probe analysis of electrode materials for Li-ion batteries: challenges and ways forward

Abstract: The worldwide developments of electric vehicles, as well as large-scale or grid-scale energy storage to compensate the intermittent nature of renewable energy generation has generated a surge of interest in...

Cited by 30 publications

References 76 publications

Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies

Enabling Extreme Fast‐Charging: Challenges at the Cathode and Mitigation Strategies

Nanoscale Compositional Mapping of Commercial LiNi0.8Co0.15Al0.05O2 Cathodes Using Atom Probe Tomography

Tracking the Mn Diffusion in the Carbon-Supported Nanoparticles Through the Collaborative Analysis of Atom Probe and Evaporation Simulation

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Product

Resources

About

Nanoscale Compositional Mapping of Commercial LiNi_0.8Co_0.15Al_0.05O₂ Cathodes Using Atom Probe Tomography